WO2021256398A1 - Batterie à semi-conducteurs - Google Patents

Batterie à semi-conducteurs Download PDF

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Publication number
WO2021256398A1
WO2021256398A1 PCT/JP2021/022312 JP2021022312W WO2021256398A1 WO 2021256398 A1 WO2021256398 A1 WO 2021256398A1 JP 2021022312 W JP2021022312 W JP 2021022312W WO 2021256398 A1 WO2021256398 A1 WO 2021256398A1
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Prior art keywords
electrode layer
solid
state battery
positive electrode
negative electrode
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PCT/JP2021/022312
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English (en)
Japanese (ja)
Inventor
廣一 中野
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株式会社村田製作所
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Priority to JP2022531771A priority Critical patent/JPWO2021256398A1/ja
Priority to CN202180042617.8A priority patent/CN115699444A/zh
Publication of WO2021256398A1 publication Critical patent/WO2021256398A1/fr
Priority to US18/062,070 priority patent/US20230100780A1/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/547—Terminals characterised by the disposition of the terminals on the cells
    • H01M50/548—Terminals characterised by the disposition of the terminals on the cells on opposite sides of the cell
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/572—Means for preventing undesired use or discharge
    • H01M50/584—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/586—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries inside the batteries, e.g. incorrect connections of electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/572—Means for preventing undesired use or discharge
    • H01M50/584—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/59—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries characterised by the protection means
    • H01M50/591—Covers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a solid state battery. More specifically, the present invention relates to a solid-state battery in which an insulating portion is laminated on the electrode layer in the boundary region between the electrode layer of the solid-state battery and the external terminal.
  • a secondary battery may be used as a power source for electronic devices such as smartphones and notebook computers.
  • a liquid electrolyte is generally used as a medium for ion transfer that contributes to charging and discharging. That is, a so-called “electrolyte” is used in the secondary battery.
  • electrolytic solution a liquid electrolyte
  • safety is generally required in terms of preventing leakage of the electrolytic solution. Further, since the organic solvent and the like used in the electrolytic solution are flammable substances, safety is also required in that respect.
  • the inventor of the present application noticed that the conventional solid-state battery had a problem to be overcome, and found that it was necessary to take measures for that purpose. Specifically, the inventor of the present application has found that there are the following problems.
  • the conventional solid-state battery 100 has at least one battery structural unit including a positive electrode layer 110, a negative electrode layer 120, and a solid electrolyte layer 130 interposed therein at least in the stacking direction. It has a solid-state battery laminate 150 provided. Further, the solid-state battery 100 includes positive electrode terminals 160A and negative electrode terminals 160B provided on opposite side surfaces or end faces (more specifically, left and right side surfaces or end faces) of the solid-state battery laminate 150 as external terminals. The positive electrode terminal 160A is electrically connected to the positive electrode layer 110, and the negative electrode terminal 160B is electrically connected to the negative electrode layer 120.
  • an insulating portion (or an insulating portion) is used to prevent an electrical short circuit between the positive electrode layer 110 and the negative electrode terminal 160B and between the negative electrode layer 120 and the positive electrode terminal 160A.
  • 140 also referred to as an electrode separation portion or a margin layer
  • each layer can be formed by firing, and it is desirable that the solid-state battery laminate forms an integrally sintered body. Therefore, the solid-state battery laminate can be used by a printing method such as a screen printing method. It is desirable to manufacture by laminating technology such as green sheet method using green sheet.
  • the positive electrode layer 110 (specifically, the paste for forming the positive electrode layer 110) rises or rises. , It becomes easy to be electrically short-circuited in the vicinity of the negative electrode layer 120 which can be formed located above the stacking direction.
  • the negative electrode layer 120 (specifically, the paste for forming the negative electrode layer 120) is raised or raised and is located above the stacking direction. It is easy to be electrically short-circuited in the vicinity of the positive electrode layer 110 that can be formed.
  • the positive electrode layer 110 (specifically, the paste for forming the positive electrode layer 110) is formed when the positive electrode layer 110 is formed by a printing method or the like. It extends toward the negative electrode terminal 160B and is close to the negative electrode terminal 160B, making it easy to short-circuit electrically.
  • the negative electrode layer 120 (specifically, the paste for forming the negative electrode layer 120) extends toward the positive electrode terminal 160A and is close to the positive electrode terminal 160A. It becomes easy to short-circuit electrically.
  • the above problem is particularly large when the electrode layer is multi-layered because the current collector layer (more specifically, the positive electrode current collector layer 211 or the like) can be arranged in the electrode layer as shown in FIG. It was also found by the research of the inventor of the present application that it became remarkable.
  • a main object of the present invention is to provide a solid-state battery in which short-circuiting between electrode layers, short-circuiting between an electrode layer and an external terminal, and peeling of the electrode layer are further suppressed.
  • a solid cell having at least one battery building block including a positive electrode layer, a negative electrode layer, and a solid electrolyte layer interposed between the positive electrode layer and the negative electrode layer, for example, along the stacking direction. It is composed of a battery laminate, and is provided with external terminals of a positive electrode terminal and a negative electrode terminal provided on opposite side surfaces (more specifically, left and right side surfaces as shown in the illustrated embodiment) of the solid battery laminate. At least one of the positive electrode layer and the negative electrode layer has a structure in which the active material portion and the insulating portion of the electrode layer are laminated with each other in the boundary region with the external terminal, and is viewed in cross section. A solid battery in which the insulating portion covers the active material portion in a sleeve shape is provided.
  • the electrode layer (1, 2) is included in at least one electrode layer (1, 2) in the boundary region X with the external terminal 6. It has a structure in which a possible active material portion (1', 2') and an insulating portion 4 or a part thereof are laminated with each other, and the insulating portion 4 is "sleeve-shaped" in a cross-sectional view. It is characterized by covering 1', 2').
  • the insulating portion 4, particularly its "sleeve-like is such that the insulating portion 4 can be arranged outside or vertically in the stacking direction of the electrode layers (1, 2).
  • the part (S) overlaps the electrode layer (1, 2), especially the active material portion (1', 2'), and above all, the main surface of the electrode layer (1, 2), especially the active material portion. It is characterized by contacting on the main surface of (1', 2').
  • FIG. 1 is a schematic cross-sectional view schematically showing a boundary region of a solid-state battery according to an embodiment of the present invention.
  • FIG. 2 is a schematic cross-sectional view schematically showing a solid-state battery according to the first embodiment of the present invention.
  • FIG. 3 is a schematic cross-sectional view schematically showing the boundary region of the solid-state battery according to the first embodiment of the present invention.
  • FIG. 4 is a schematic cross-sectional view schematically showing the solid-state battery according to the second embodiment of the present invention.
  • FIG. 5 is a schematic cross-sectional view schematically showing the boundary region of the solid-state battery according to the second embodiment of the present invention.
  • FIG. 6 is a schematic cross-sectional view schematically showing the solid-state battery according to the third embodiment of the present invention.
  • FIG. 7 is a schematic cross-sectional view schematically showing the boundary region of the solid-state battery according to the third embodiment of the present invention.
  • FIG. 8 is a schematic cross-sectional view schematically showing the solid-state battery according to the fourth embodiment of the present invention.
  • FIG. 9 is a schematic cross-sectional view schematically showing the boundary region of the solid-state battery according to the fourth embodiment of the present invention.
  • FIG. 10 is a schematic view schematically showing the formation of the insulating portion.
  • FIG. 11 is a schematic diagram schematically showing the formation of another insulating portion.
  • FIG. 12 is a schematic cross-sectional view schematically showing a conventional solid-state battery.
  • FIG. 13 is a schematic cross-sectional view schematically showing another conventional solid-state battery.
  • solid-state battery of the present invention will be described in detail. Although the description will be given with reference to the drawings as necessary, the contents illustrated are merely schematically and exemplary for the understanding of the present invention, and the appearance and / or the dimensional ratio may differ from the actual product. ..
  • the "cross-sectional view” referred to in the present specification is based on a form when viewed from a direction substantially perpendicular to the thickness direction based on the stacking direction or the stacking direction of each layer that can constitute a solid-state battery. In other words, it is based on the form when cut out on a plane parallel to the thickness direction. In short, it is based on the form of the cross section of the object shown in FIGS. 1 and 2, for example.
  • the "vertical direction” and “horizontal direction” used directly or indirectly in the present specification correspond to the vertical direction and the horizontal direction in the figure, respectively. Unless otherwise specified, the same sign or symbol shall indicate the same member or part or the same meaning.
  • the vertical downward direction that is, the direction in which gravity acts
  • the opposite direction corresponds to the "upward direction” / "top surface side”. Can be done.
  • the “solid-state battery” as used in the present invention refers to a battery whose components can be composed of a solid in a broad sense, and in a narrow sense, an all-solid-state battery in which its components (particularly preferably all components) can be composed of a solid. Pointing to.
  • the solid-state battery in the present invention is a laminated solid-state battery in which the layers forming the battery building unit are laminated to each other, and preferably such layers are made of a sintered body.
  • the "solid-state battery” may include not only a so-called “secondary battery” that can be repeatedly charged and discharged, but also a "primary battery” that can only be discharged.
  • a “solid-state battery” is a secondary battery.
  • the "secondary battery” is not overly bound by its name and may include, for example, a power storage device.
  • the solid-state battery comprises at least an electrode layer of a positive electrode and a negative electrode and a solid electrolyte layer (or a solid electrolyte). More specifically, for example, as shown in FIG. 2, a solid-state battery has a positive electrode layer (1), a negative electrode layer (2), and a solid electrolyte layer (or solid electrolyte) (3) at least interposed between them. It comprises a solid-state battery laminate (5) including at least one battery building block along the stacking direction.
  • each layer that can form the solid-state battery may be formed by firing, and the positive electrode layer, the negative electrode layer, the solid electrolyte layer, and the like may form a sintered layer. More preferably, the positive electrode layer, the negative electrode layer and the solid electrolyte layer are each integrally fired, and therefore the battery building block or the solid-state battery laminate may form an integrally sintered body.
  • the positive electrode layer (1) is an electrode layer containing at least a positive electrode active material. Therefore, the positive electrode layer (1) may be a positive electrode active material layer mainly composed of a positive electrode active material. The positive electrode layer may further contain a solid electrolyte, if necessary. In some embodiments, the positive electrode layer may be composed of a sintered body containing at least positive electrode active material particles and solid electrolyte particles.
  • the negative electrode layer (2) is an electrode layer including at least a negative electrode active material. Therefore, the negative electrode layer (2) may be a negative electrode active material layer mainly composed of a negative electrode active material. The negative electrode layer may further contain a solid electrolyte, if necessary. In some embodiments, the negative electrode layer may be composed of a sintered body containing at least negative electrode active material particles and solid electrolyte particles.
  • the positive electrode active material and the negative electrode active material are substances that can be involved in the occlusion and release of ions and the transfer of electrons to and from an external circuit in a solid-state battery. Ions move (conduct) between the positive electrode layer and the negative electrode layer via the solid electrolyte.
  • the occlusion and release of ions to the active material involves the oxidation or reduction of the active material, and the electrons or holes for such a redox reaction move from the external circuit to the external terminal and further to the positive electrode layer or the negative electrode layer. Charging and discharging can proceed by the delivery.
  • the positive and negative layers are, for example, lithium ion, sodium ion, proton (H + ), potassium ion (K + ), magnesium ion (Mg 2+ ), aluminum ion (Al 3+ ), silver ion (Ag + ), and fluoride.
  • Examples of the positive electrode active material that can be contained in the positive electrode layer (1) include a lithium-containing phosphoric acid compound having a pearcon-type structure, a lithium-containing phosphoric acid compound having an olivine-type structure, a lithium-containing layered oxide, and a spinel-type structure. Examples thereof include at least one selected from the group consisting of lithium-containing oxides and the like.
  • the lithium-containing phosphoric acid compound having a pear-con type structure Li 3 V 2 (PO 4 ) 3 and the like can be mentioned.
  • lithium-containing phosphoric acid compounds having an olivine-type structure examples include Li 3 Fe 2 (PO 4 ) 3 , LiFePO 4 , LiMnPO 4 , and / or LiFe 0.6 Mn 0.4 PO 4 .
  • lithium-containing layered oxides include LiCoO 2 , LiCo 1/3 Ni 1/3 Mn 1/3 O 2 , and / or LiCo 0.8 Ni 0.15 Al 0.05 O 2 .
  • lithium-containing oxides having a spinel-type structure include LiMn 2 O 4 and / or LiNi 0.5 Mn 1.5 O 4 and the like.
  • the positive electrode active material capable of occluding and releasing sodium ions includes a sodium-containing phosphoric acid compound having a nacicon-type structure, a sodium-containing phosphoric acid compound having an olivine-type structure, a sodium-containing layered oxide, and sodium having a spinel-type structure. At least one selected from the group consisting of oxides and the like can be mentioned.
  • Examples of the negative electrode active material that can be contained in the negative electrode layer (2) include oxides and carbon materials such as graphite containing at least one element selected from the group consisting of Ti, Si, Sn, Cr, Fe, Nb and Mo. , At least selected from the group consisting of graphite-lithium compounds, lithium alloys, lithium-containing phosphoric acid compounds having a pearcon-type structure, lithium-containing phosphoric acid compounds having an olivine-type structure, lithium-containing oxides having a spinel-type structure, and the like. There is one kind. Examples of lithium alloys include Li-Al and the like.
  • lithium-containing phosphoric acid compounds having a pearcon-type structure examples include Li 3 V 2 (PO 4 ) 3 and / or LiTi 2 (PO 4 ) 3 .
  • lithium-containing phosphoric acid compounds having an olivine-type structure examples include Li 3 Fe 2 (PO 4 ) 3 and / or LiCuPO 4 .
  • Li 4 Ti 5 O 12 and the like can be mentioned.
  • the negative electrode active material that can occlude and release sodium ions includes a group consisting of a sodium-containing phosphoric acid compound having a nacicon-type structure, a sodium-containing phosphoric acid compound having an olivine-type structure, and a sodium-containing oxide having a spinel-type structure. At least one selected from is mentioned.
  • the positive electrode layer and the negative electrode layer may be made of the same material.
  • the positive electrode layer and / or the negative electrode layer may contain a conductive material.
  • the conductive material that can be contained in the positive electrode layer and the negative electrode layer include at least one selected from the group consisting of metal materials such as silver, palladium, gold, platinum, aluminum, copper and nickel, and carbon. Can be done.
  • the positive electrode layer and / or the negative electrode layer may contain a sintering aid.
  • a sintering aid at least one selected from the group consisting of lithium oxide, sodium oxide, potassium oxide, boron oxide, silicon oxide, bismuth oxide and phosphorus oxide can be mentioned.
  • the thickness of the positive electrode layer and the negative electrode layer is not particularly limited.
  • the thickness of each of the positive electrode layer and the negative electrode layer may be 2 ⁇ m or more and 100 ⁇ m or less, and particularly may be 5 ⁇ m or more and 50 ⁇ m or less.
  • the solid electrolyte (or solid electrolyte layer) (3) is a material capable of conducting ions such as lithium ion or sodium ion.
  • the solid electrolyte forming a battery constituent unit in a solid-state battery may form, for example, a layer in which lithium ions can be conducted between the positive electrode layer and the negative electrode layer.
  • Specific examples of the solid electrolyte include a lithium-containing phosphoric acid compound having a pearcon-type structure, an oxide having a perovskite-type structure, an oxide having a garnet-type or garnet-type similar structure, and an oxide glass ceramics-based lithium ion conductor. And so on.
  • Li x M y (PO 4 ) 3 (1 ⁇ x ⁇ 2,1 ⁇ y ⁇ 2, M is a group consisting of Ti, Ge, Al, Ga, and Zr It is at least one of the more selected).
  • Li 1.2 Al 0.2 Ti 1.8 (PO 4 ) 3 and the like can be mentioned.
  • an oxide having a perovskite-type structure La 0.55 Li 0.35 TiO 3 and the like can be mentioned.
  • oxides having a garnet-type or garnet-type similar structure include Li 7 La 3 Zr 2 O 12 and the like.
  • oxide glass ceramics-based lithium ion conductor for example, a phosphoric acid compound (LATP) containing lithium, aluminum and titanium as a constituent element, and a phosphoric acid compound (LAGP) containing lithium, aluminum and germanium as constituent elements are used.
  • LATP phosphoric acid compound
  • LAGP phosphoric acid compound
  • the solid electrolyte in which sodium ions can be conducted include sodium-containing phosphoric acid compounds having a pearcon-type structure, oxides having a perovskite-type structure, oxides having a garnet-type or garnet-type similar structure, and the like.
  • the sodium-containing phosphate compound having a NASICON-type structure Na x M y (PO 4 ) 3 (1 ⁇ x ⁇ 2,1 ⁇ y ⁇ 2, M is a group consisting of Ti, Ge, Al, Ga, and Zr It is at least one of the more selected).
  • the solid electrolyte layer may contain a sintering aid.
  • the sintering aid that may be contained in the solid electrolyte layer may be selected from, for example, the same materials as the sintering aid that may be contained in the positive electrode layer and / or the negative electrode layer.
  • the thickness of the solid electrolyte layer is not particularly limited.
  • the thickness of the solid electrolyte layer may be, for example, 1 ⁇ m or more and 15 ⁇ m or less, and particularly may be 1 ⁇ m or more and 5 ⁇ m or less.
  • the positive electrode layer (1) and the negative electrode layer (2) may include a positive electrode current collector layer and a negative electrode current collector layer, respectively.
  • the positive electrode current collector layer and the negative electrode current collector layer may each have the form of a foil.
  • the positive electrode current collector layer and the negative electrode current collector layer may have the form of a sintered body.
  • the positive electrode current collector layer and / or the negative electrode current collector layer has the form of a sintered body, it may be composed of a sintered body containing a conductive material and / or a sintering aid.
  • the conductive material that can be contained in the positive electrode current collector and / or the negative electrode current collector layer may be selected from, for example, the same materials as the conductive material that can be contained in the positive electrode layer and / or the negative electrode layer.
  • the sintering aid that may be contained in the positive electrode current collector layer and / or the negative electrode current collector layer may be selected from, for example, the same materials as the sintering aid that may be contained in the positive electrode layer and / or the negative electrode layer.
  • the thickness of the positive electrode current collector layer and the negative electrode current collector layer is not particularly limited.
  • the thickness of each of the positive electrode current collector layer and the negative electrode current collector layer may be 1 ⁇ m or more and 10 ⁇ m or less, and particularly may be 1 ⁇ m or more and 5 ⁇ m or less.
  • the positive electrode current collector layer and / or the negative electrode current collector layer is not indispensable, and a solid-state battery in which such a positive electrode current collector layer and / or a negative electrode current collector layer is not provided is also considered. Be done. That is, the solid-state battery in the present invention may be a “current collector-less” solid-state battery (see FIG. 2).
  • the solid-state battery laminate (5) is provided with terminals for connection with the outside (hereinafter, referred to as "external terminal” or “external terminal 6").
  • terminals for connecting to the outside are provided as "end face electrodes" on the side surfaces (specifically, the left and right side surfaces) of the solid-state battery laminate (5).
  • the external terminal 6 for example, as shown in FIG. 2, the positive electrode side terminal (positive electrode terminal) (6A) electrically connected to the positive electrode layer (1), the negative electrode layer (2), and electricity.
  • the terminal on the negative electrode side (negative electrode terminal) (6B) connected to the solid-state battery may be provided in the solid-state battery laminate 5.
  • Such terminals preferably include a material (or a conductive material) having a high conductivity.
  • the material of the terminal is not particularly limited, and examples thereof include at least one selected from the group consisting of gold, silver, platinum, aluminum, tin, nickel, copper, manganese, cobalt, iron, titanium and chromium. be able to.
  • the position where the terminals are arranged is not particularly limited, and is not limited to the left and right sides of the solid-state battery laminate.
  • FIG. 1 shows a solid-state battery according to an embodiment of the present invention (hereinafter, may be referred to as “the solid-state battery of the present disclosure”).
  • the solid-state battery of the present disclosure includes, for example, as shown in FIG. 1, at least two electrode layers (1, 2) having different polarities, and a solid electrolyte layer 3 intervening at least between the electrode layers (1, 2). It comprises a solid-state battery laminate comprising at least one battery building block along the stacking direction (see FIG. 2).
  • the solid-state battery of the present disclosure includes an external terminal 6 (positive electrode terminal or negative electrode terminal).
  • an external terminal 6 positive electrode terminal or negative electrode terminal.
  • a positive electrode terminal 6A and a negative electrode terminal 6B provided on opposite side surfaces (specifically, left and right side surfaces) of the solid-state battery laminate 5 as shown in FIG. 2 are provided.
  • the electrode layer (1, 2) may be contained in the electrode layer (1, 2) in the boundary region X with the external terminal 6, the active material portion (1'). , 2') and the insulating portion 4 (or a part thereof) may be laminated with each other in the vertical direction, and the insulating portion 4 is "sleeve-shaped" in the cross-sectional view of the active material portion (1'). , 2') is covered.
  • the electrode layer 1 is shown as a positive electrode layer and the electrode layer 2 is shown as a negative electrode layer in FIG. 1, but the electrode layer 1 may be a negative electrode layer, and therefore the electrode layer 2 may be a positive electrode layer. .. That is, although the external terminal 6 is shown as a positive electrode terminal for convenience of explanation, the external terminal 6 may be a positive electrode terminal or a negative electrode terminal.
  • the "active material portion” means a portion of the electrode layer containing the electrode active material. More specifically, it means a portion of the positive electrode layer containing at least the above-mentioned “positive electrode active material” and a portion of the negative electrode layer containing at least the above-mentioned “negative electrode active material”.
  • the "boundary region” means a region in which the "electrode layer” and the “external terminal” can be arranged so as to face each other, and in this boundary region, the "electrode layer” and the “external terminal” are electrically connected to each other. It may or may not be electrically connected.
  • an "insulation portion" can be arranged in such a boundary region. Therefore, in the solid-state battery of the present disclosure, a region in which such an "insulating portion" can be arranged can also be referred to as a "boundary region”.
  • the boundary region X exists in a region where the external terminals 6 (for example, positive electrode terminals) can be arranged so as to face each other.
  • the electrode layer 1 and the external terminal 6 are electrically connected, and the electrode layer 2 and the external terminal 6 are not electrically connected via the insulating portion 4.
  • the "insulating portion” (also referred to as “electrode separation portion” or “margin” or “margin layer”) means that at least the electrode layer (positive electrode layer and / or negative electrode layer) and the external terminal face each other. It means a region where the electrode layer can be arranged, that is, a region where the electrode layer can be arranged at the boundary region with the external terminal, and the electrode layer and the external terminal can be separated and / or electrically insulated. Specifically, it means a portion that separates and / or electrically insulates the electrode layer and the external terminal in the direction in which the positive electrode terminal and the negative electrode terminal of the solid-state battery face each other or in the left-right direction.
  • the material that can form the insulating part is not particularly limited, but it is preferable that the material is composed of, for example, the above-mentioned "solid electrolyte” or "insulating material".
  • the "insulating material” examples include glass materials and ceramic materials.
  • the "glass material” is not particularly limited, but is, for example, soda lime glass, potash glass, borate glass, borosilicate glass, barium borate glass, borate subsalt glass, borate. Selected from the group consisting of barium-based glass, bismuth borosilicate-based glass, bismuth-zinc borate glass, bismuth-silicate-based glass, phosphate-based glass, aluminophosphate-based glass, and phosphate sub-salt-based glass. At least one type can be mentioned.
  • the “ceramic material” is not particularly limited, and is, for example, aluminum oxide (Al 2 O 3 ), boron nitride (BN), silicon dioxide (SiO 2 ), silicon nitride (Si 3 N 4 ), and zirconium oxide. At least one selected from the group consisting of (ZrO 2 ), aluminum nitride (AlN), silicon carbide (SiC) and barium titanate (BaTIO 3) can be mentioned.
  • the solid electrolyte material that can be contained in the insulating portion is the same material as the solid electrolyte that can be contained in the above-mentioned "solid electrolyte layer". With such a configuration, the bondability between the insulating portion and the solid electrolyte layer can be further improved.
  • the solid-state battery of the present disclosure for example, as shown in FIG. 1, at least one of two electrode layers (specifically, a positive electrode layer 1 and a negative electrode layer 2) has an external terminal 6 (specifically, a positive electrode terminal).
  • the active material portion (1', 2') contained in the electrode layers (1, 2) and the insulating portion 4 (or a part thereof) are laminated with each other in the vertical direction. Therefore, the main feature is that the insulating portion 4 covers the active material portion (1', 2') in a "sleeve-like" (sleeve-like) manner in a cross-sectional view.
  • the electrode layer covered with the sleeve-shaped portion of the insulating portion in cross-sectional view is the active material portion.
  • the “sleeve-like” portion of the insulating portion 4 is indicated by the reference numeral “S” (Sleeve), and the other “non-sleeve-like” portion is indicated by the reference numeral “NS” (Non-Sleeve). show.
  • the sleeve-shaped portion (S) of the insulating portion 4 is provided so as to sandwich the active material portion (1', 2') from above and below in the stacking direction in a cross-sectional view. ..
  • the sleeve-shaped portion (S) of the insulating portion 4 is arranged so as to sandwich the active material portion (1', 2') of the electrode layer (1, 2) from above and below.
  • the sleeve-shaped portion (S) of the insulating portion 4 has, for example, a shape like a robot arm, a crab claw, or a beak in a cross-sectional view. ..
  • the sleeve-shaped portion (S) is shown in a rectangular or rectangular shape in a cross-sectional view, but the sleeve-shaped portion (S) and the active material portion (1', 2') are shown.
  • the boundary with and may be a gentle curve, may be curved inward, may be curved outward, may be fillet-shaped, and may be tapered and narrowed as it approaches the external terminal 6. It may have such a shape.
  • the active material portion (1', 2') of the electrode layer (1, 2) is vertically (or or) particularly at the time of manufacturing the solid-state battery laminate. Extension (exudation, protrusion) in the stacking direction), particularly proximity to electrode layers having different polarities can be suppressed, and short-circuiting between electrode layers facing each other in the stacking direction can be further prevented after manufacturing.
  • the active material portion 2'of the electrode layer 2 can be moved in the left-right direction (or the positive electrode terminal and the negative electrode terminal), especially when the solid-state battery laminate is manufactured. Extension (exudation, protrusion) in the opposite direction), particularly proximity to the external terminal 6 can be further suppressed, and short-circuiting of the electrode layer 2 with the opposite external terminal 6 can be further prevented after manufacturing. can.
  • the contact area of the insulating portion 4 with the solid electrolyte layer 3 is further secured, and the electrode is used during the manufacturing of the solid-state battery or the charging / discharging of the solid-state battery. It is possible to further suppress peeling at the interface of the layers (1, 2), specifically, peeling from the solid electrolyte layer, particularly delamination.
  • the sleeve-shaped portion (S) of the insulating portion 4 with respect to the thickness of the electrode layers (1, 2) (specifically, the dimension in the stacking direction (vertical direction)).
  • the dimension in the left-right direction thereof) ratio is, for example, 0.05% or more and 10% or less.
  • the length of the portion where the sleeve-shaped portion of the insulating portion 4 (S) are duplicated, the length of the positive and negative terminals and the direction opposite (left-right direction) indicated by the distance D 1 in the cross-sectional view of FIG. 1 For example, it is 10 ⁇ m or more and 200 ⁇ m or less, preferably 30 ⁇ m or more and 50 ⁇ m or less.
  • the thickness (T s ) of the sleeve-shaped portion (S) of the insulating portion 4 is, for example, 1% or more and 50% or less (T s / T 3 ⁇ 100 ) with respect to the thickness (T 3 ) of the solid electrolyte layer 3. (%)). Since the shape of the cross section of the sleeve-shaped portion (S) may be a shape other than a rectangle or a rectangle, the thickness (Ts ) of the sleeve-shaped portion (S ) is defined as the “average thickness” of the sleeve-shaped portion (S).
  • the active material portion 1' is the external terminal 6 (specifically, the positive electrode terminal).
  • the electrode layer 1 may be electrically connected to the external terminal 6. That is, an electrical "connection state" may be formed.
  • the active material portion 2' is an external terminal 6 (specifically, a positive electrode layer 2) as shown in, for example, the electrode layer 2 (specifically, the negative electrode layer 2). It does not have to extend to the terminal), and the electrode layer 2 does not have to be electrically connected to the external terminal 6. That is, the insulating portion 4 may form an electrical "non-connected state".
  • the electrical connection with the external terminal of the electrode layer can be arbitrarily selected.
  • FIG. 2 shows the solid-state battery 10 of the first embodiment.
  • the solid-state battery 10 shown in FIG. 2 has at least one battery structural unit including a positive electrode layer 1, a negative electrode layer 2, and a solid electrolyte layer 3 interposed between the positive electrode layer 1 and the negative electrode layer 2 at least in the stacking direction. It has a solid-state battery laminate 5 provided.
  • the solid-state battery 10 includes external terminals of a positive electrode terminal 6A and a negative electrode terminal 6B provided on opposite side surfaces (specifically, left and right side surfaces) of the solid-state battery laminate 5.
  • at least one of the electrode layers of the positive electrode layer 1 and the negative electrode layer 2 is the active material of the electrode layer (1, 2) in the boundary region (X a , X b) with the external terminals (6A, 6B).
  • the portion (1', 2') and the insulating portion (or a part thereof) are laminated in the vertical direction, and the insulating portion is sleeve-shaped in the cross-sectional view of the active material portion (1', 2').
  • the main feature is that it covers 2').
  • the insulating portion 4a of the positive electrode side is present in the boundary region X a of the positive electrode terminal 6A.
  • the positive electrode layer 1 (or the active material portion 1') is electrically connected to the positive electrode terminal 6A. More specifically, the positive electrode layer 1 extends through the inside (inside) of the insulating portion 4a and is electrically connected to the positive electrode terminal 6A (formation of a connected state).
  • the insulating portion 4b on the negative electrode side also exists in the boundary region Xb with the negative electrode terminal 6B, and the positive electrode layer 1 is not electrically connected to the negative electrode terminal 6B (non-connected state). Formation).
  • the same insulating portions 4 (upper and lower) as shown in FIG. 1 can be used.
  • the negative electrode layer 2 is electrically connected to the negative electrode terminal 6B in the boundary region Xb with the negative electrode terminal 6B.
  • the active material portion 2 of the negative electrode layer 2 ' is not connected to positive terminal 6A electrically ( Formation of a disconnected state).
  • the same insulating portion 4 as that shown in FIG. 1 (lower stage) can be used.
  • an insulating portion on the negative electrode side may be provided as in the insulating portion 4a on the positive electrode side.
  • the negative electrode layer 2 may extend inside (inside) the insulating portion (not shown) on the negative electrode side and electrically connect to the negative electrode terminal 6B (formation of a connected state).
  • the sleeve-shaped portion of the insulating portion and the electrode layer are flush with each other in a cross-sectional view. ..
  • the sleeve-shaped portion (S) of the insulating portion 4a and the positive electrode layer 1 Is preferably flush with the portion (F) not covered by the insulating portion 4a.
  • the sleeve-shaped portion (S) of the insulating portion 4 and the negative electrode layer 2 are preferably flush with each other.
  • the thickness of each layer can be made uniform, so that the structural stability of the solid-state battery is further improved. Further, by making the thickness of each layer uniform, delamination at the interface between the electrode layer and the solid electrolyte layer can be further suppressed.
  • the length of the sleeve-shaped portion (S) of the insulating portion 4 with respect to the thickness of the electrode layers (1, 2) (specifically, the dimension in the stacking direction (vertical direction)) in the cross-sectional view.
  • the ratio (length / thickness ratio) of the (specifically, the dimension in the left-right direction thereof) is, for example, 0.05% or more and 10% or less.
  • the sleeve-shaped portion (S) of the insulating portion 4a of the positive electrode layer 1 and the sleeve-shaped portion (S) of the insulating portion 4 of the negative electrode layer 2 overlap in the stacking direction (vertical direction).
  • the distance D 1 of the overlapping portion is, for example, 10 ⁇ m or more and 200 ⁇ m or less, preferably 30 ⁇ m or more and 50 ⁇ m or less, as the length in the direction (left-right direction) in which the positive electrode terminal and the negative electrode terminal of the solid-state battery 10 face each other.
  • the total length of the sleeve-shaped portion (S) and the non-sleeve-shaped portion (NS) is not particularly limited.
  • the negative electrode is used.
  • Layer 2 may be longer.
  • the insulating portions of the positive electrode layer 1 and the negative electrode layer 2 may have the same length.
  • an electrical short circuit between the electrode layers (1 and 2) that is, a short circuit in the vertical direction
  • electrical short circuit that is, short circuit in the left-right direction
  • the solid-state battery 20 of the second embodiment is shown in FIGS. 4 and 5.
  • the configuration of the solid-state battery 20 of the second embodiment is the same as the configuration of the solid-state battery 10 of the first embodiment, but the solid-state battery 20 of the second embodiment is provided with the positive electrode layer 21 including the positive electrode current collecting layer 21c. It is different from the solid-state battery 10.
  • the positive electrode current collector layer 21c extends so as to pass between the sleeve-shaped insulating portions 24a in a cross-sectional view, and particularly through the sleeveless portion (NS) of the insulating portion 24a with the positive electrode terminal 26A. It is electrically connected (Fig. 5).
  • the solid-state battery 20 may include a negative electrode current collector layer in the negative electrode layer 22 as well as the positive electrode layer 21 (not shown).
  • the length of the sleeve-shaped portion (S) with respect to the thickness of the electrode layer (21, 22) (specifically, the dimension in the stacking direction (vertical direction)) (specifically).
  • the ratio (length / thickness ratio) of the dimension in the left-right direction is, for example, 0.05% or more and 10% or less.
  • the sleeve-shaped portion (S) of the insulating portion 24a of the positive electrode layer 21 and the sleeve-shaped portion (S) of the insulating portion 24 of the negative electrode layer 22 are in the stacking direction (vertical direction). It is preferable to overlap in.
  • the distance D 2 of the overlapping portion is, for example, 10 ⁇ m or more and 200 ⁇ m or less, preferably 30 ⁇ m or more and 50 ⁇ m or less, as the length in the direction (left-right direction) in which the positive electrode terminal and the negative electrode terminal face each other.
  • the insulating portions 24a and 24b of the positive electrode layer 21 and the insulating portion 24 of the negative electrode layer 22 have the same configuration as the insulating portions (4a, 4b, 4) of the solid-state battery 10 of the first embodiment.
  • the electrode layer (21, 22) includes a current collector layer, that is, even if the electrode layer is multi-layered, the electrode layer (21) , 22), an electrical short circuit between the negative electrode layer 22 and the positive electrode terminal 26A, and an electrical short circuit between the positive electrode layer 21 and the negative electrode terminal 26B (that is, left and right).
  • Directional short circuit), delamination between the electrode layer (21, 22) and the solid electrolyte layer 23, etc. can be suppressed in the same manner.
  • FIGS. 6 and 7 show the solid-state battery 30 of the third embodiment.
  • the configuration of the solid-state battery 30 of the third embodiment is the same as the configuration of the solid-state battery 20 of the second embodiment, but the solid-state battery 30 of the third embodiment has the insulating portions 34a and 34b of the positive electrode layer 31 and the negative electrode layer 32. It differs from the solid-state battery 20 in that the shape of the insulating portion 34 of the above is changed.
  • the sleeve-shaped portion of the insulating portion is raised, raised, or higher than the portion where the electrode layer (or the active material portion) is not covered with the insulating portion. ..
  • the sleeve-shaped portion (S) of the insulating portion 34a of the positive electrode layer 31 is the insulating portion 34a of the positive electrode layer 31 (or the active material portion (31')). It is raised, raised or raised above the uncovered portion (F). More specifically, the sleeve-shaped portion (S) is raised, raised, or raised in the vertical direction in the stacking direction.
  • the sleeve-shaped portion (S) of the insulating portion 34 of the negative electrode layer 32 is raised or raised more than the portion (F) in which the negative electrode layer 32 (or the active material portion (32')) is not covered with the insulating portion 34. It is exciting or high.
  • the sleeve-shaped portion (S) is raised, raised, or raised in the vertical direction in the stacking direction.
  • the sleeve-shaped portion (S) is shown to be raised in a rectangular or rectangular shape due to a step in a cross-sectional view, but an arc is drawn with a gentle curve or a curved surface. It may be raised or raised or raised.
  • the thickness (T 3S ) of the sleeve-shaped portion (S) is, for example, 1% or more and 50% or less with respect to the thickness (T 31 , T 32 ) of the portion (F) not covered by the insulating portion of the electrode layer. It is raised at a height in the range (T 3S / T 31 or T 32 ⁇ 100 (%)).
  • the thickness (T 3S ) of the sleeve-shaped portion (S) is raised or raised at a height in the range of, for example, 1% or more and 50% or less with respect to the thickness (T 33 ) of the solid electrolyte layer 33. Or it is higher (T 3S / T 33 ⁇ 100 (%)).
  • the thickness (T 3s ) of the sleeve-shaped portion (S) may be different or the same.
  • the raised sleeve-shaped portion of the insulating portion is raised, raised or raised more than the portion in contact with the external terminal of the insulating portion in the cross-sectional view.
  • the sleeve-shaped portion (S) with respect to the thickness of the electrode layer (31, 32) (specifically, the dimension (T 31 , T 32) in the stacking direction (vertical direction)) in the cross-sectional view. ) (Specifically, the dimension in the left-right direction thereof) ratio (length / thickness ratio) is, for example, 0.05% or more and 10% or less.
  • the sleeve-shaped portion (S) of the insulating portion 34a of the positive electrode layer 31 and the sleeve-shaped portion (S) of the insulating portion 34 of the negative electrode layer 32 overlap in the stacking direction (vertical direction).
  • the distance D 3 of the overlapping portion is, for example, 10 ⁇ m or more and 200 ⁇ m or less, preferably 30 ⁇ m or more and 50 ⁇ m or less, as the length in the direction (left-right direction) in which the positive electrode terminal and the negative electrode terminal face each other.
  • the sleeve-shaped portion (S) is raised so that an electrical short circuit (that is, a short circuit in the vertical direction) between the electrode layers (31, 32) and a negative electrode layer are performed.
  • the sleeve-shaped portion (S) is raised, so that the filling amount of the active material in each electrode layer is increased. Can be further increased, so that the energy density can be further improved.
  • the lower side (lower surface) of the insulating portion is covered with a sleeve shape of the electrode layer as in the first and second embodiments (see FIGS. 1 to 5). It may be flush with the non-existing portion (F).
  • the configuration of the solid-state battery 40 of the fourth embodiment is the same as the configuration of the solid-state battery 30 of the third embodiment, but the solid-state battery 40 of the fourth embodiment has the insulating portions 44a and 44b of the positive electrode layer 41 and the negative electrode layer 42. It differs from the solid-state battery 30 in that the shape of the insulating portion 44 of the above, particularly the shape of the "non-sleeve-shaped portion" is changed.
  • the sleeve-shaped portion of the insulating portion is raised, raised, or higher than the portion where the electrode layer (or the active material portion) is not covered with the insulating portion. ..
  • the sleeve-shaped portion (S) of the insulating portion 44a of the positive electrode layer 41 is the insulating portion 44a of the positive electrode layer 41 (or the active material portion (41')). It is raised, raised or raised above the uncovered portion (F).
  • the sleeve-shaped portion (S) of the insulating portion 44 of the negative electrode layer 42 is raised more than the portion (F) in which the negative electrode layer 42 (or the active material portion (42')) is not covered with the insulating portion 44.
  • the sleeve-shaped portion (S) is shown to be raised in a rectangular or rectangular shape due to a step in a cross-sectional view, but an arc is drawn with a gentle curve or a curved surface. It may be raised.
  • the thickness (T 4S ) of the sleeve-shaped portion (S) is, for example, 1% or more and 50% or less with respect to the thickness (T 41 , T 42 ) of the portion (F) not covered by the insulating portion of the electrode layer. It is raised, raised or raised at a range height (T 4S / T 41 or T 42 x 100 (%)).
  • the thickness (T 4S ) of the sleeve-shaped portion (S) is raised or raised at a height in the range of, for example, 1% or more and 50% or less with respect to the thickness (T 43 ) of the solid electrolyte layer 43. Or it is higher (T 4S / T 43 ⁇ 100 (%)).
  • the thickness (T 4s ) of the sleeve-shaped portion (S) may be different or the same.
  • the raised sleeve-shaped portion of the insulating portion is flush with the portion where the insulating portion contacts the external terminal in a cross-sectional view.
  • the raised sleeve-shaped portion (S) of the insulating portion 44a of the positive electrode layer 41 comes into contact with the positive electrode terminal 46A of the insulating portion 44a. It is preferable that the portion (specifically, the end portion in contact with the positive electrode terminal 46A on the right side of the sleeveless portion (NS)) is flush with or has the same height. Further, in a cross-sectional view, the raised sleeve-shaped portion (S) of the insulating portion 44 of the negative electrode layer 42 is in contact with the positive electrode terminal 46A of the insulating portion 44 (specifically, the non-sleeve-shaped portion (NS). ) Is flush with the end portion in contact with the positive electrode terminal 46A on the right side, or the height is matched and coincides with each other.
  • the sleeve-shaped portion (S) with respect to the thickness of the electrode layer (41, 42) (specifically, the dimension (T 41 , T 42) in the stacking direction (vertical direction)) in the cross-sectional view. ) (Specifically, the dimension in the left-right direction thereof) ratio (length / thickness ratio) is, for example, 0.05% or more and 10% or less.
  • the sleeve-shaped portion (S) of the insulating portion 44a of the positive electrode layer 41 and the sleeve-shaped portion (S) of the insulating portion 44 of the negative electrode layer 42 overlap in the stacking direction (that is, the vertical direction).
  • the distance D 4 of the overlapping portion is, for example, 10 ⁇ m or more and 200 ⁇ m or less, and 30 ⁇ m or more and 50 ⁇ m or less as the length in the direction in which the positive electrode terminal and the negative electrode terminal face each other or in the left-right direction.
  • the sleeve-shaped portion (S) is raised, raised, or raised, so that an electrical short circuit (that is, that is) between the electrode layers (41, 42) is performed.
  • an electrical short circuit that is, that is
  • Vertical short circuit electrical short circuit between the negative electrode layer 42 and the positive electrode terminal 46A, electrical short circuit between the positive electrode layer 41 and the negative electrode terminal 46B (that is, short circuit in the left and right direction), electrode layer (41, 42). Delamination between the solid electrolyte layer 43 and the like can be further suppressed.
  • the thickness of the sleeveless portion (NS) of the insulating portion is increased as compared with the solid-state battery of the first to third embodiments, so that the negative electrode layer 42 and the positive electrode terminal are increased. It is possible to further suppress an electrical short circuit with the 46A and an electrical short circuit between the positive electrode layer 41 and the negative electrode terminal 46B (that is, a short circuit in the left-right direction).
  • the lower side (lower surface) of the insulating portion is a sleeve-shaped portion of each electrode layer as in the first and second embodiments (see FIGS. 1 to 5). It may be flush with the portion (F) not covered with.
  • the solid-state battery of the present disclosure may be a combination of the configurations of the first to fourth embodiments described above as necessary, and in particular, the insulating portions used in the first to fourth embodiments are appropriately used. It may be used in combination.
  • the solid-state battery of the present disclosure is not limited to the above embodiment.
  • the solid-state battery laminate can be produced by a printing method such as a screen printing method, a green sheet method using a green sheet, or a composite method thereof. That is, the solid-state battery laminate itself may be manufactured according to a conventional solid-state battery manufacturing method (therefore, the solid electrolyte, the organic binder, the solvent, any additive, the positive electrode active material, and the negative electrode active material described below. As the raw material such as, those used in the manufacture of known solid-state batteries may be used).
  • (Laminate block formation) Prepare a slurry by mixing solid electrolytes, organic binders, solvents and optional additives. Then, a sheet having a thickness of about 10 ⁇ m after firing is obtained by sheet molding from the prepared slurry. -Mix a positive electrode active material, a solid electrolyte, a conductive material, an organic binder, a solvent and any additive to prepare a positive electrode paste. Similarly, the negative electrode active material, the solid electrolyte, the conductive material, the organic binder, the solvent and any additive are mixed to prepare a paste for the negative electrode. -Print the positive electrode paste on the sheet, and print the current collector layer as needed.
  • the negative electrode paste is printed on the sheet, and the current collector layer is printed if necessary.
  • -A sheet on which the positive electrode paste is printed and a sheet on which the negative electrode paste is printed are alternately laminated to obtain a laminate.
  • the outermost layer (top layer and / or bottom layer) of the laminate even if it is an electrolyte layer, it is an insulating layer (a layer that does not conduct electricity, for example, a non-conductive material such as a glass material and / or a ceramic material). It may be a layer that can be constructed), or it may be an electrode layer.
  • the external terminal (or end face electrode) on the positive electrode side can be formed by applying a conductive paste to the exposed side surface of the positive electrode in the sintered laminate.
  • the external terminal (or end face electrode) on the negative electrode side can be formed by applying a conductive paste to the exposed side surface of the negative electrode in the sintered laminate.
  • the external terminals on the positive electrode side and the negative electrode side are not limited to being formed after sintering the laminated body, but may be formed before firing and subjected to simultaneous sintering.
  • the insulating portion can be formed, for example, as follows, if necessary, in the above-mentioned "layered block formation" (before firing).
  • a solid electrolyte and / or an insulating material, a binder, an organic binder, a solvent and any additive are mixed to prepare an insulating paste (also referred to as an electrode separation paste or a margin paste).
  • the insulating portion 24a having the shape shown in FIG. 5 (upper row) can be formed according to, for example, the procedure shown in FIG. (A)
  • the insulating paste P 2 is printed on the sheet P 1 formed from the slurry containing the solid electrolyte. At this time, it is preferable to print the insulating paste P 2 so that a desired “sleeve-like” portion is formed.
  • the current collector layer (paste) P 4 is printed on the entire surfaces of the paste P 2 and the paste P 3.
  • the electrode paste P 5 is printed on the current collector layer P 4 (the electrode paste P 5 has the same polarity as the electrode paste P 3). In this case it is preferable to print the electrode paste P 5 as desired portions of the "shaped sleeve” may be formed.
  • the paste P 6 is preferably the same as the paste P 2.
  • the insulating portion having the shape shown in FIG. 5 (upper row) can be finally formed by firing, but the formation of the insulating portion is not limited by the above method.
  • the insulating portion 24 having the shape shown in FIG. 5 can be formed according to, for example, the procedure shown in FIG. (A)
  • the insulating paste Q 2 is printed on the sheet Q 1 formed from the slurry containing the solid electrolyte. At this time, it is preferable to print the insulating paste so that a desired "sleeve-like" portion can be formed.
  • C Some of the paste Q 2 and paste Q 3 to print an insulating paste Q 4 in (where covered by part of the "sleeve").
  • the paste Q 4 is preferably the same as the paste Q 2.
  • the insulating portion having the shape shown in FIG. 5 (lower stage) can be finally formed by firing.
  • the formation of the insulating portion is not limited by the above method.
  • the insulating part By forming the insulating part according to the above procedure, various variations of the insulating part can be formed.
  • the method for manufacturing the solid-state battery is not limited to the above-mentioned manufacturing method.
  • the solid-state battery of the present invention can be used in various fields where battery use or storage can be expected. Although only an example, the solid-state battery of the present invention is used in the fields of electricity, information, and communication (for example, mobile phones, smartphones, laptop computers and digital cameras, activity meters, arm computers, etc.) in which electric / electronic devices can be used.
  • the solid-state battery of the present invention is used in the fields of electricity, information, and communication (for example, mobile phones, smartphones, laptop computers and digital cameras, activity meters, arm computers, etc.) in which electric / electronic devices can be used.
  • Electrical / electronic equipment field or mobile equipment field including electronic paper, wearable devices, RFID tags, card-type electronic money, small electronic devices such as smart watches), household / small industrial applications (for example, electric tools, golf carts, households)
  • Industrial robots for / nursing / industrial robots large industrial applications (eg forklifts, elevators, bay port cranes), transportation systems (eg hybrid cars, electric cars, buses, trains, electric assisted bicycles, electric) (Fields such as motorcycles), power system applications (for example, various power generation, road conditioners, smart grids, general home-installed power storage systems, etc.), medical applications (medical equipment fields such as earphone hearing aids), pharmaceutical applications (dose management) It can be used in fields such as systems), IoT fields, and space / deep sea applications (for example, fields such as space explorers and submersible research vessels).

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Abstract

L'invention concerne une batterie à semi-conducteurs. L'invention concerne une batterie à semi-conducteurs comprenant un stratifié de batterie à semi-conducteurs comprenant au moins une unité constitutive de batterie comprenant : une couche d'électrode positive, une couche d'électrode négative et une couche d'électrolyte solide interposée entre la couche d'électrode positive et la couche d'électrode négative. Ladite batterie à semi-conducteurs comprend des bornes externes d'une borne d'électrode positive et d'une borne d'électrode négative disposées respectivement sur des surfaces latérales opposées du stratifié de batterie à semi-conducteurs. Au moins une couche d'électrode de la couche d'électrode positive et de la couche d'électrode négative est conçue de sorte qu'une partie de matériau actif et une partie d'isolation de la couche d'électrode soient stratifiées l'une sur l'autre dans une région de limite entre la couche d'électrode et la borne externe. Dans une vue en coupe transversale, la partie d'isolation recouvre la partie de matériau actif sous une forme de manchon.
PCT/JP2021/022312 2020-06-15 2021-06-11 Batterie à semi-conducteurs WO2021256398A1 (fr)

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US18/062,070 US20230100780A1 (en) 2020-06-15 2022-12-06 Solid state battery

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WO2012164642A1 (fr) * 2011-05-27 2012-12-06 トヨタ自動車株式会社 Batterie bipolaire entièrement monolithique
JP2015133178A (ja) * 2014-01-09 2015-07-23 日産自動車株式会社 電極、および電極を有する電池
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JP2012038425A (ja) * 2010-08-03 2012-02-23 Toyota Motor Corp 電極体の製造方法及び電極体
WO2012164642A1 (fr) * 2011-05-27 2012-12-06 トヨタ自動車株式会社 Batterie bipolaire entièrement monolithique
JP2015133178A (ja) * 2014-01-09 2015-07-23 日産自動車株式会社 電極、および電極を有する電池
WO2017073164A1 (fr) * 2015-10-30 2017-05-04 ブラザー工業株式会社 Unité d'électrode, batterie et procédé de fabrication d'unité d'électrode
JP2019197652A (ja) * 2018-05-09 2019-11-14 トヨタ自動車株式会社 積層電池の製造方法

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